Charge Instability in Single-Layer TiTe_{2} Mediated by van der Waals Bonding to Substrates.

Single layers of transition metal dichalcogenides are of interest for emergent properties; an often-neglected issue is substrate effects. Our experiments show that the charge density wave in a single-layer TiTe_{2} grown on PtTe_{2} films is strongly suppressed by increasing the PtTe_{2} substrate thickness. Given that the interfacial bonding remains of the weak incommensurate van der Waals type, the observed changes are correlated with a thickness-dependent metallicity transformation in the PtTe_{2} substrate. The results illustrate the crucial role of the substrate in single-layer physics.

Dimensionality-Mediated Semimetal-Semiconductor Transition in Ultrathin PtTe_{2} Films.

Platinum ditelluride (PtTe_{2}), a type-II Dirac semimetal, remains semimetallic in ultrathin films down to just two triatomic layers (TLs) with a negative gap of -0.36 eV. Further reduction of the film thickness to a single TL induces a Lifshitz electronic transition to a semiconductor with a large positive gap of +0.79 eV. This transition is evidenced by experimental band structure mapping of films prepared by layer-resolved molecular beam epitaxy, and by comparing the data to first-principles calculations using a hybrid functional. The results demonstrate a novel electronic transition at the two-dimensional limit through film thickness control.

Massive Suppression of Proximity Pairing in Topological (Bi_{1-x}Sb_{x})_{2}Te_{3} Films on Niobium.

Interfacing bulk conducting topological Bi_{2}Se_{3} films with s-wave superconductors initiates strong superconducting order in the nontrivial surface states. However, bulk insulating topological (Bi_{1-x}Sb_{x})_{2}Te_{3} films on bulk Nb instead exhibit a giant attenuation of surface superconductivity, even for films only two layers thick. This massive suppression of proximity pairing is evidenced by ultrahigh-resolution band mappings and by contrasting quantified superconducting gaps with those of heavily n-doped topological Bi_{2}Se_{3}/Nb. The results underscore the limitations of using superconducting proximity effects to realize topological superconductivity in nearly intrinsic systems.

Unique Gap Structure and Symmetry of the Charge Density Wave in Single-Layer VSe_{2}.

Single layers of transition metal dichalcogenides (TMDCs) are excellent candidates for electronic applications beyond the graphene platform; many of them exhibit novel properties including charge density waves (CDWs) and magnetic ordering. CDWs in these single layers are generally a planar projection of the corresponding bulk CDWs because of the quasi-two-dimensional nature of TMDCs; a different CDW symmetry is unexpected. We report herein the successful creation of pristine single-layer VSe_{2}, which shows a (sqrt[7]×sqrt[3]) CDW in contrast to the (4×4) CDW for the layers in bulk VSe_{2}. Angle-resolved photoemission spectroscopy from the single layer shows a sizable (sqrt[7]×sqrt[3]) CDW gap of ∼100 meV at the zone boundary, a 220 K CDW transition temperature twice the bulk value, and no ferromagnetic exchange splitting as predicted by theory. This robust CDW with an exotic broken symmetry as the ground state is explained via a first-principles analysis. The results illustrate a unique CDW phenomenon in the two-dimensional limit.

Reduction of Intrinsic Electron Emittance from Photocathodes Using Ordered Crystalline Surfaces.

The generation of intense electron beams with low emittance is key to both the production of coherent x rays from free electron lasers, and electron pulses with large transverse coherence length used in ultrafast electron diffraction. These beams are generated today by photoemission from disordered polycrystalline surfaces. We show that the use of single crystal surfaces with appropriate electronic structures allows us to effectively utilize the physics of photoemission to generate highly directed electron emission, thus reducing the emittance of the electron beam being generated.

Topological phases in double layers of bismuthene and antimonene.

Two-dimensional topological insulators show great promise for spintronic applications. Much attention has been placed on single atomic or molecular layers, such as bismuthene. The selections of such materials are, however, limited. To broaden the base of candidate materials with desirable properties for applications, we report herein an exploration of the physics of double layers of bismuthene and antimonene. The electronic structure of a film depends on the number of layers, and it can be modified by epitaxial strain, by changing the effective spin-orbit coupling strength, and by the manner in which the layers are geometrically stacked. First-principles calculations for the double layers reveal a number of phases, including topological insulators, topological semimetals, Dirac semimetals, trivial semimetals, and trivial insulators. Their phase boundaries and the stability of the phases are investigated. The results illustrate a rich pattern of phases that can be realized by tuning lattice strain and effective spin-orbit coupling.

Dimensional Effects on the Charge Density Waves in Ultrathin Films of TiSe2.

Charge density wave (CDW) formation in solids is a critical phenomenon involving the collective reorganization of the electrons and atoms in the system into a wave structure, and it is expected to be sensitive to the geometric constraint of the system at the nanoscale. Here, we study the CDW transition in TiSe2, a quasi-two-dimensional layered material, to determine the effects of quantum confinement and changing dimensions in films ranging from a single layer to multilayers. Of key interest is the characteristic length scale for the transformation from a two-dimensional case to the three-dimensional limit. Angle-resolved photoemission spectroscopy (ARPES) measurements of films with thicknesses up to six layers reveal substantial variations in the energy structure of discrete quantum well states; however, the temperature-dependent band gap renormalization converges at just three layers. The results indicate a layer-dependent mixture of two transition temperatures and a very-short-range CDW interaction within a three-dimensional framework.

Proving Nontrivial Topology of Pure Bismuth by Quantum Confinement.

The topology of pure Bi is controversial because of its very small (∼10 meV) band gap. Here we perform high-resolution angle-resolved photoelectron spectroscopy measurements systematically on 14-202 bilayer Bi films. Using high-quality films, we succeed in observing quantized bulk bands with energy separations down to ∼10 meV. Detailed analyses on the phase shift of the confined wave functions precisely determine the surface and bulk electronic structures, which unambiguously show nontrivial topology. The present results not only prove the fundamental property of Bi but also introduce a capability of the quantum-confinement approach.

Photoemission Circular Dichroism and Spin Polarization of the Topological Surface States in Ultrathin Bi2Te3 Films.

Circular dichroism (CD) observed by photoemission, being sensitive to the orbital and spin angular momenta of the electronic states, is a powerful probe of the nontrivial surface states of topological insulators, but the experimental results thus far have eluded a comprehensive description. We report a study of Bi2Te3 films with thicknesses ranging from one quintuple layer (two-dimensional limit) to 12 layers (bulk limit) over a wide range of incident photon energy. The data show complex variations in magnitude and sign reversals, which are nevertheless well described by a theoretical calculation including all three photoemission mechanisms: dipole transition, surface photoemission, and spin-orbit coupling. The results establish the nontrivial connection between the spin-orbit texture and CD.

Surface Collective Modes in the Topological Insulators Bi_{2}Se_{3} and Bi_{0.5}Sb_{1.5}Te_{3-x}Se_{x}.

We used low-energy, momentum-resolved inelastic electron scattering to study surface collective modes of the three-dimensional topological insulators Bi_{2}Se_{3} and Bi_{0.5}Sb_{1.5}Te_{3-x}Se_{x}. Our goal was to identify the "spin plasmon" predicted by Raghu and co-workers [Phys. Rev. Lett. 104, 116401 (2010)]. Instead, we found that the primary collective mode is a surface plasmon arising from the bulk, free carriers in these materials. This excitation dominates the spectral weight in the bosonic function of the surface χ^{"}(q,ω) at THz energy scales, and is the most likely origin of a quasiparticle dispersion kink observed in previous photoemission experiments. Our study suggests that the spin plasmon may mix with this other surface mode, calling for a more nuanced understanding of optical experiments in which the spin plasmon is reported to play a role.

Electronic size effects in three-dimensional nanostructures.

We show that bismuth nanostructures form three-dimensional patterns governed by two-dimensional electronic effects. Scanning tunneling microscopy reveals that both the vertical and the lateral dimensions of the structures strongly favor certain values and that the preferred widths are substantially different for each preferred height. First-principles calculations demonstrate that this vertical-lateral correlation is governed by the Fermi surface topology and that this is itself sensitively dependent on the dimensions of the structure.

Interfacial bonding and structure of Bi2Te3 topological insulator films on Si(111) determined by surface x-ray scattering.

Interfacial topological states are a key element of interest for topological insulator thin films, and their properties can depend sensitively on the atomic bonding configuration. We employ in situ nonresonant and resonant surface x-ray scattering to study the interfacial and internal structure of a prototypical topological film system: Bi2Te3 grown on Si(111). The results reveal a Te-dominated buffer layer, a large interfacial spacing, and a slightly relaxed and partially strained bottom quintuple layer of an otherwise properly stacked bulklike Bi2Te3 film. The presence of the buffer layer indicates a nontrivial process of interface formation and a mechanism for electronic decoupling between the topological film and the Si(111) substrate.

Fragility of surface states and robustness of topological order in Bi2Se3 against oxidation.

Topological surface states are protected against local perturbations, but this protection does not extend to chemical reaction over the whole surface, as demonstrated by theoretical studies of the oxidation of Bi(2)Se(3) and its effects on the surface spin polarization and current. While chemisorption of O(2) largely preserves the topological surface states, reaction with atomic O removes the original surface states and yields two new sets of surface states. One set forms a regular Dirac cone but is topologically trivial. The other set, while topologically relevant, forms an unusual rounded Dirac cone. The details are governed by the hybridization interaction at the interface.

Interfacial protection of topological surface states in ultrathin Sb films.

Spin-polarized gapless surface states in topological insulators form chiral Dirac cones. When such materials are reduced to thin films, the Dirac states on the two faces of the film can overlap and couple by quantum tunneling, resulting in a thickness-dependent insulating gap at the Dirac point. Calculations for a freestanding Sb film with a thickness of four atomic bilayers yield a gap of 36 meV, yet angle-resolved photoemission measurements of a film grown on Si(111) reveal no gap formation. The surprisingly robust Dirac cone is explained by calculations in terms of interfacial interaction.

Illuminating the surface spin texture of the giant-Rashba quantum-well system Bi/Ag(111) by circularly polarized photoemission.

We have mapped out the spin texture of a Bi/Ag surface alloy prepared on a thin Ag film by circularly polarized angle-resolved photoemission spectroscopy. A term proportional to ∇·A in the interaction Hamiltonian gives rise to strong surface photoexcitation, which interferes with a Rashba contribution to yield a pronounced circular dichroic effect in Bi/Ag. The dipole transition, often taken to be the only important photoexcitation mechanism, is actually negligible. A parameter-free calculation yields a dichroic pattern in excellent agreement with experiment.

Controlling the topology of Fermi surfaces in metal nanofilms.

The properties of metal crystals are governed by the electrons of the highest occupied states at the Fermi level and determined by Fermi surfaces, the Fermi energy contours in momentum space. Topological regulation of the Fermi surface has been an important issue in synthesizing functional materials, which we found to be realized at room temperature in nanometer-thick films. Reducing the thickness of a metal thin film down to its electron wavelength scale induces the quantum size effect and the electronic system changes from three to two-dimensional, transforming the Fermi surface topology. Such an ultrathin film further changes its topology through one-dimensional (1D) structural deformation of the film when it is grown on a 1D substrate. In particular, when the interface has 1D metallic bands, the system is additionally stabilized by forming an electron energy gap by hybridization between 1D states of the film and substrate.

Passage from spin-polarized surface states to unpolarized quantum well states in topologically nontrivial Sb films.

Topological materials have unusual surface spin properties including a net surface spin current protected by the bulk symmetry properties. When such materials are reduced to thin films, their gapless spin-polarized surface states must connect, by analytic continuation, to bulk-derived quantum-well states, which are spin-unpolarized in centrosymmetric systems. The nature of this passage in a model system, Sb films, is investigated. Angle-resolved photoemission shows a smooth transition, while calculations elucidate the correlated evolution of the spin and charge distributions in real space.

Visualizing electronic chirality and Berry phases in graphene systems using photoemission with circularly polarized light.

Electronic chirality near the Dirac point is a key property of graphene systems, which is revealed by the spectral intensity patterns as measured by angle-resolved photoemission spectroscopy under various polarization conditions. Specifically, the strongly modulated circular patterns for monolayer (bilayer) graphene rotate by ±90° (±45°) in changing from linearly to circularly polarized light; these angles are directly related to the phases of the wave functions and thus visually confirm the Berry's phase of π (2π) around the Dirac point. The details are verified by calculations.

Coherent Electronic Band Structure of TiTe2/TiSe2 Moiré Bilayer.

A van der Waals bonded moiré bilayer formed by sequential growth of TiSe2 and TiTe2 monolayers exhibits emergent electronic structure as evidenced by angle-resolved photoemission band mapping. The two monolayers adopt the same lattice orientation but incommensurate lattice constants. Despite the lack of translational symmetry, sharp dispersive bands are observed. The dispersion relations appear distinct from those for the component monolayers alone. Theoretical calculations illustrate the formation of composite bands by coherent electronic coupling despite the weak interlayer bonding, which leads to band renormalization and energy shifts.